三维立体介孔结构的海藻酸钠/氧化石墨烯复合气凝胶的制备及其对亚甲基蓝的吸附

朱薇; 江坤; 游峰; 姚楚; 王昆; 江学良

doi:10.13801/j.cnki.fhclxb.20210730.001

三维立体介孔结构的海藻酸钠/氧化石墨烯复合气凝胶的制备及其对亚甲基蓝的吸附

doi: 10.13801/j.cnki.fhclxb.20210730.001

朱薇^{1, 2},
江坤^{1, 3},
游峰^{1, 3},
姚楚^{1, 3},
王昆²,
江学良^{1, 3, ,}

1.
武汉工程大学材料科学与工程学院，武汉 430074
2.
武汉工程大学邮电与信息工程学院，武汉 430073
3.
武汉工程大学湖北省等离子化学与新材料重点实验室，武汉 430073

基金项目: 国家自然科学基金 (51273154)；湖北省自然科学基金 (2017CFB289)；湖北省教育厅科研项目 (B2016483)；等离子体化学与新材料湖北省重点实验室创新基金 (2020CX03)

详细信息

通讯作者:
江学良，博士，教授，博士生导师，研究方向为有机-无机杂化材料与功能高分子材料　E-mail：jiangxl@wit.edu.cn

中图分类号: TB3333
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出版历程
- 收稿日期: 2021-05-17
- 修回日期: 2021-06-23
- 录用日期: 2021-07-09
- 网络出版日期: 2021-07-30
- 刊出日期: 2022-03-23

Preparation of 3-dimensional mesoporous sodium alginate/graphene oxide composite aerogel for adsorption of methylene blue

ZHU Wei^{1, 2},
JIANG Kun^{1, 3},
YOU Feng^{1, 3},
YAO Chu^{1, 3},
WANG Kun²,
JIANG Xueliang^{1, 3
, ,}

1.
School of Material Science and Engineering, Wuhan Institute of Technology, Wuhan 430073, China
2.
College of Post and Telecommunication of WIT, Wuhan 430073, China
3.
Hubei Key Laboratory of Plasma Chemistry and New Materials, Wuhan Institute of Technology, Wuhan 430073, China

摘要

摘要: 为了有效去除废水中的染料，本论文以海藻酸钠 (SA) 和氧化石墨烯 (GO) 为原料，采用一步水热法制备海藻酸钠/氧化石墨烯 (SA/GO) 复合水凝胶，并通过冷冻干燥法得SA/GO复合气凝胶。利用FT-IR、XRD、SEM、TEM、N₂等温吸附-脱附、接触角来表征SA/GO复合气凝胶并研究其吸附性能。结果表明，SA/GO复合气凝胶是具有三维立体结构的多孔材料，BET比表面积约为580.54 m²·g⁻¹。讨论了SA/GO复合气凝胶对亚甲基蓝 (MB) 溶液吸附过程的影响因素，在碱性条件下，吸附效果最好，吸附率可达99.41%，吸附量可达248.53 mg·g⁻¹，并表现出优异的循环再生性。
- 氧化石墨烯 /
- 海藻酸钠 /
- 亚甲基蓝 /
- 吸附 /
- 循环 /
- 复合气凝胶
Abstract: In order to effectively remove dye from wastewater, sodium alginate/graphene oxide (SA/GO) compo-site hydrogel was prepared by one-step hydrothermal method using sodium alginate (SA) and graphene oxide (GO) as raw materials, and SA/GO composite aerogel was prepared by freeze drying. The synthesized products were characterized by FT-IR, XRD, SEM, TEM, N₂ adsorption-desorption and contact angel. The results show that the SA/GO composite aerogel is a porous material with three-dimensional structure, the specific surface area is about 580.54 m²·g⁻¹. The influence factors of SA/GO composite aerogel on the adsorption process of methylene blue (MB) solution are discussed. Under alkaline conditions, the adsorption effect is the best, the adsorption rate can reach 99.41%, the adsorption capacity can reach 248.53 mg·g⁻¹, and show excellent cyclic regeneration.
- graphene oxide /
- sodium alginate /
- methylene blue /
- adsorption /
- recycle /
- composite aerogel

HTML全文

图 1 不同样品的FT-IR光谱图: (a) 氧化石墨烯 (GO) 气凝胶; (b) 海藻酸钠/氧化石墨烯 (SA/GO) 复合气凝胶

Figure 1. FT-IR spectra of different samples: (a) Graphene oxide (GO) aerogel; (b) Sodium alginate/graphene oxide (SA/GO) composite aerogel

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图 2 不同样品的XRD图谱：(a) GO气凝胶; (b) SA/GO 复合气凝胶

Figure 2. XRD patterns of different samples: (a) GO aerogel; (b) SA/GO composite aerogel

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图 3 GO气凝胶和SA/GO复合气凝胶的SEM ((a), (b)) 和SA/GO复合气凝胶的TEM图像 ((c), (d)）

Figure 3. SEM images of samples for GO aerogel and SA/GO composite aerogel ((a), (b)), TEM images of SA/GO composite aerogel ((c), (d))

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图 4 SA/GO复合气凝胶的N₂吸附-解吸曲线 (a) 以及BJH孔径分布曲线 (b)

Figure 4. N₂ adsorption-desorption curve (a) and BJH pore size distribution curve (b) of SA/GO composite aerogel

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图 5 GO气凝胶 (a) 和SA/GO复合气凝胶 (b) 的接触角

Figure 5. Contact angles of GO aerogel (a) and SA/GO composite aeroge (b)

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图 6 GO气凝胶与SA/GO复合气凝胶对亚甲基蓝 (MB) 吸附性能的比较

Figure 6. Comparison of adsorption properties of GO aerogel and SA/GO composite aerogel for methylene blue (MB)

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图 7 染料浓度对SA/GO复合气凝胶吸附MB性能的影响

Figure 7. Effect of dye concentration on MB adsorption performance of SA/GO composite aerogel

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图 8 吸附剂原料比例对SA/GO复合气凝胶吸附MB性能的影响

Figure 8. Effect of proportion of adsorbent materials on MB adsorption performance of SA/GO composite aerogel

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图 9 pH值对SA/GO复合气凝胶吸附MB性能的影响

Figure 9. Effect of pH on MB adsorption performance of SA/GO composite aerogel

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图 10 SA/GO复合气凝胶对不同染料的吸附性能

Figure 10. Adsorption properties of SA/GO composite aerogel on different dyes

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图 11 SA/GO复合气凝胶对MB的循环吸附性

Figure 11. Cyclic adsorption of SA/GO composite aerogels on MB

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图 12 SA/GO复合气凝胶吸附MB的Langmuir吸附等温线 (a) 和Freundlich吸附等温线 (b)

Figure 12. Langmuir adsorption isotherm (a) and Freundlich adsorption isotherm (b) of SA/GO composite aerogels on MB

C_e—Concentration at adsorption equilibrium; Q_e—Adsorption capacity at adsorption equilibrium

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图 13 SA/GO复合气凝胶吸附MB的准一级吸附动力学 (a) 和准二级吸附动力学(b)模型

Figure 13. Quasi-first-order adsorption kinetics (a) and quasi-secondary adsorption kinetic model (b) of SA/GO composite aerogels on MB

t—Adsorption time; q_t—Adsorption capacity at time t

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图 14 SA/GO复合气凝胶吸附原理图

Figure 14. Schematic diagram of adsorption by SA/GO composite aerogel

MB—Methylene blue；RhB—Rhodamine B

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表 1 SA/GO复合气凝胶的孔结构分析

Table 1. Hole structure analysis of SA/GO composite aerogel

Parameter	BET/ (m²·g⁻¹)	Pore diameter/ nm	Pore volume/ (cm³·g⁻¹)
Value	580.54	3.41	0.40

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表 2 Langmuir和Freundlich等温吸附参数

Table 2. Isothermal adsorption parameters of Langmuir and Freundlich

T/℃	Langmuir				Freundlich
T/℃	Q_max/(mg·g⁻¹)	K_L/(L·mg⁻¹)	R_L	R²	k_F/(mg·g⁻¹·(L·mg⁻¹)^1/n)	n	R²
25	207.9002	1.6141	0.0122	0.98421	246.3985	3.7158	0.99775
Notes: Q_max—Saturated adsorption capacity; K_L—Langmuir constant; R_L—Dimensionless equilibrium parameters; R²—Fitting constant; k_F—Freundlich constants related to adsorption capacity; n—Freundlich constants related to adsorption strength; T—Temperature.

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表 3 MB吸附动力学模型拟合结果

Table 3. MB Kinetic model parameters of adsorption

Model	R²	q_e	k
Quasi-first-order adsorption kinetics model	0.99397	27.8477	0.03671
Quasi-secondary adsorption kinetics model	0.99982	253.1646	0.00395
Notes: R²—Fitting constant; q_e—Equilibrium adsorption capacity; k—Adsorption kinetics constant.

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表 4 各种吸附剂对MB吸附能力的比较

Table 4. Adsorption performance of different adsorbents for MB

Adsorbents	Maximum adsorption capacity/(mg·g⁻¹)	Ref.	Date/year
Carboxymethyl cellulose/carboxylated graphene oxide composite microbeads	180.23	[33]	2020
Pineapple peel carboxy methylcellulose-g-poly(acryliccid-co-acrylamide)/graphene oxide hydrogels	133.32	[34]	2019
Reduced graphene oxide and montmorillonite composite aerogel	227.27	[35]	2018
Graphene oxide-magnetic iron oxide nanoparticles	232.56	[36]	2018
Manganese ferrite-graphene oxide nanocomposites	177.30	[37]	2018
SA/GO composite aerogel	248.53	This study

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